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卤代醇的电化学去质子化能够实现用于捕获 CO 并将其转化为碳酸亚乙酯的级联反应。

Electrochemical deprotonation of halohydrins enables cascading reactions for CO capture and conversion into ethylene carbonate.

作者信息

Kim Jeong Hyun, Jo Young In, Jang Jun Ho, Yu Hyun Ji, Kim Jeong Eun, Kim Hyun Jae, Yeo Jia Bin, Lee Moo Young, Nam Ki Tae

机构信息

Department of Materials Science and Engineering, Seoul National University, Seoul, Republic of Korea.

出版信息

Nat Commun. 2025 May 30;16(1):5038. doi: 10.1038/s41467-025-60354-8.

DOI:10.1038/s41467-025-60354-8
PMID:40447599
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12125186/
Abstract

Electrochemical processes for CO mitigation can be broadly categorized into two approaches: CO capture via electrochemically generated bases and CO conversion through electrochemical reduction. Recent advancements have been concentrated to developing methods that efficiently capture and release CO or reduce base-CO adducts while regenerating bases for subsequent CO capture. In this study, we introduce an electrochemical strategy that integrates CO capture and conversion through a series of domino reactions initiated by the electrochemical generation of organic bases. This method involves the electrochemical deprotonation of halohydrin molecules, which generate hydrogen and halo-alkoxides that capture CO and spontaneously undergo intramolecular cyclization to yield cyclic carbonates. Direct and indirect Faradaic efficiency of up to 100% is achieved for both hydrogen and ethylene carbonate production, demonstrating highly selective sequential capture and conversion reactions. Our system provides a scalable pathway for synthesizing various cyclic carbonates directly from diluted CO sources.

摘要

用于减少二氧化碳的电化学过程大致可分为两种方法

通过电化学产生的碱捕获二氧化碳以及通过电化学还原转化二氧化碳。最近的进展主要集中在开发能够有效捕获和释放二氧化碳或还原碱 - 二氧化碳加合物,同时再生碱以便后续捕获二氧化碳的方法。在本研究中,我们介绍了一种电化学策略,该策略通过由有机碱的电化学产生引发的一系列多米诺反应来整合二氧化碳的捕获和转化。该方法涉及卤代醇分子的电化学去质子化,生成氢气和卤代醇盐,它们捕获二氧化碳并自发进行分子内环化生成环状碳酸酯。氢气和碳酸亚乙酯生产的直接和间接法拉第效率均高达100%,证明了高度选择性的顺序捕获和转化反应。我们的系统为直接从稀释的二氧化碳源合成各种环状碳酸酯提供了一条可扩展的途径。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/db50fb9b18a9/41467_2025_60354_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/390b8d01c63b/41467_2025_60354_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/e5e34a2c70c6/41467_2025_60354_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/04bd02f846ab/41467_2025_60354_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/fb4b4c9c7e30/41467_2025_60354_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/db50fb9b18a9/41467_2025_60354_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/390b8d01c63b/41467_2025_60354_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/e5e34a2c70c6/41467_2025_60354_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/04bd02f846ab/41467_2025_60354_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/fb4b4c9c7e30/41467_2025_60354_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/f466/12125186/db50fb9b18a9/41467_2025_60354_Fig5_HTML.jpg

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Metal free synthesis of ethylene and propylene carbonate from alkylene halohydrin and CO at room temperature.室温下由卤代醇和一氧化碳无金属合成碳酸亚乙酯和碳酸亚丙酯
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